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On the Additive Microstructure in Composite Cathodes and Alumina-Coated Carbon Microwires for Improved All-Solid-State Batteries

Randau, Simon and Walther, Felix and Neumann, Anton and Schneider, Yannik and Negi, Rajendra S. and Mogwitz, Boris and Sann, Joachim and Becker-Steinberger, Katharina and Danner, Timo and Hein, Simon and Latz, Arnulf and Richter, Felix H. and Janek, Jürgen (2021) On the Additive Microstructure in Composite Cathodes and Alumina-Coated Carbon Microwires for Improved All-Solid-State Batteries. Chemistry of Materials, 33 (4), pp. 1380-1393. ACS Publications. doi: 10.1021/acs.chemmater.0c04454. ISSN 0897-4756.

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Official URL: https://pubs.acs.org/doi/10.1021/acs.chemmater.0c04454


All-solid-state batteries promise to enable lithium metal anodes and outperform state-of-the-art lithium-ion battery technology. To achieve high battery capacity, utilization of the active material in the cathode must be maximized. Carbon-based conductive additives are known to improve the capacity and rate performance of electrode composites. However, their influence on cathode composites in all-solid-state batteries is yet not fully understood. Here, we study the influence of several carbon additives with different morphologies and surface areas on the performance of an all-solid-state battery cell Li|β-Li3PS4|Li(Ni0.6Co0.2Mn0.2)O2/β-Li3PS4/carbon. Cycling tests and microstructure-resolved simulations show that higher utilization of the cathode active material can be achieved using fiber-shaped vapor-grown carbon additives, whereas particle-shaped carbons show a minor influence. Unfortunately, carbon additives generally lead to an accelerated capacity loss during cycling and an enhanced formation of solid electrolyte decomposition products. The latter was studied in more detail using cyclic voltammetry, X-ray photoelectron spectroscopy, and cycling experiments. The results show that carbon additives with a small surface area and a fiber-like morphology result in the lowest degree of decomposition. To completely overcome electrolyte degradation caused by the use of carbon additives, a protection concept is developed. A thin alumina coating with a few nanometers thickness was deposited on the carbon fibers by atomic layer deposition, which successfully prevents decomposition reactions, reduces long-term capacity fading, and leads to an enhanced overall all-solid-state battery performance.

Item URL in elib:https://elib.dlr.de/144984/
Document Type:Article
Title:On the Additive Microstructure in Composite Cathodes and Alumina-Coated Carbon Microwires for Improved All-Solid-State Batteries
AuthorsInstitution or Email of AuthorsAuthor's ORCID iD
Randau, SimonJustus-Liebig-Universität GießenUNSPECIFIED
Walther, FelixJustus-Liebig-Universität GießenUNSPECIFIED
Neumann, AntonAnton.Neumann (at) dlr.dehttps://orcid.org/0000-0002-4575-8697
Schneider, YannikJustus-Liebig-Universität GießenUNSPECIFIED
Negi, Rajendra S.Justus-Liebig-Universität GießenUNSPECIFIED
Mogwitz, BorisJustus-Liebig-Universität GießenUNSPECIFIED
Sann, JoachimJustus-Liebig-Universität GießenUNSPECIFIED
Becker-Steinberger, KatharinaKatharina.Becker-Steinberger (at) dlr.deUNSPECIFIED
Danner, TimoTimo.Danner (at) dlr.dehttps://orcid.org/0000-0003-2336-6059
Hein, SimonSimon.Hein (at) dlr.dehttps://orcid.org/0000-0002-6728-9983
Latz, ArnulfArnulf.Latz (at) dlr.deUNSPECIFIED
Richter, Felix H.Justus-Liebig-Universität GießenUNSPECIFIED
Janek, JürgenJustus-Liebig-Universität GießenUNSPECIFIED
Date:11 February 2021
Journal or Publication Title:Chemistry of Materials
Refereed publication:Yes
Open Access:No
Gold Open Access:No
In ISI Web of Science:Yes
DOI :10.1021/acs.chemmater.0c04454
Page Range:pp. 1380-1393
Publisher:ACS Publications
Keywords:all-solid-state batteries conductive additives modeling simulation composite electrode
HGF - Research field:Energy
HGF - Program:Materials and Technologies for the Energy Transition
HGF - Program Themes:Electrochemical Energy Storage
DLR - Research area:Energy
DLR - Program:E SP - Energy Storage
DLR - Research theme (Project):E - Electrochemical Storage
Location: Ulm
Institutes and Institutions:Institute of Engineering Thermodynamics > Computational Electrochemistry
Deposited By: Danner, Timo
Deposited On:23 Dec 2021 20:34
Last Modified:23 Dec 2021 20:34

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